Despite the title, the album is not a collection of live duet performances by Harry Belafonte and Makeba. It is a studio album of 12 tracks, five by Belafonte, five by Makeba, and two duets. The songs are all African traditional tunes sung in tribal languages like Xhosa and Zulu.

In the mid-1960s, Belafonte was very active in supporting emerging African artists as well as making African music known worldwide, and this album is an example of this activity. It includes classical African songs like Malaika (with the English title My Angel) as well as songs in African languages such as Zulu, Sotho and Swahili.